Isolated Electron Trap-Induced Charge Accumulation for Efficient Photocatalytic Hydrogen Production

Wenhuan Huang; Chenyang Su; Chen Zhu; Tingting Bo; Shouwei Zuo; Wei Zhou; Yuanfu Ren; Yanan Zhang; Jing Zhang; Magnus Rueping; Huabin Zhang

doi:10.1002/anie.202304634

Isolated Electron Trap-Induced Charge Accumulation for Efficient Photocatalytic Hydrogen Production

Wenhuan Huang, Chenyang Su, Chen Zhu, Tingting Bo, Shouwei Zuo, Wei Zhou, Yuanfu Ren, Yanan Zhang, Jing Zhang, Magnus Rueping^*, Huabin Zhang^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

88 Scopus citations

Abstract

The solar-driven evolution of hydrogen from water using particulate photocatalysts is considered one of the most economical and promising protocols for achieving a stable supply of renewable energy. However, the efficiency of photocatalytic water splitting is far from satisfactory due to the sluggish electron-hole pair separation kinetics. Herein, isolated Mo atoms in a high oxidation state have been incorporated into the lattice of Cd_0.5Zn_0.5S (CZS@Mo) nanorods, which exhibit photocatalytic hydrogen evolution rate of 11.32 mmol g⁻¹ h⁻¹ (226.4 μmol h⁻¹; catalyst dosage 20 mg). Experimental and theoretical simulation results imply that the highly oxidized Mo species lead to mobile-charge imbalances in CZS and induce the directional photogenerated electrons transfer, resulting in effectively inhibited electron-hole recombination and greatly enhanced photocatalytic efficiency.

Original language	English (US)
Article number	e202304634
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	25
DOIs	https://doi.org/10.1002/anie.202304634
State	Published - Jun 19 2023

Bibliographical note

Funding Information:
This work received financial support from the King Abdullah University of Science and Technology (KAUST), National Natural Science Foundation of China (22001156, 22271178), International Cooperation Key Project of Science and Technology Department of Shaanxi, China (2022KWZ‐06), the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province (20210602), Research project of Xi′an Science and Technology Bureau (2022GXFW0011), and Science and Technology New Star in Shaanxi Province (2023KJXX‐045).

Funding Information:
This work received financial support from the King Abdullah University of Science and Technology (KAUST), National Natural Science Foundation of China (22001156, 22271178), International Cooperation Key Project of Science and Technology Department of Shaanxi, China (2022KWZ-06), the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province (20210602), Research project of Xi′an Science and Technology Bureau (2022GXFW0011), and Science and Technology New Star in Shaanxi Province (2023KJXX-045).

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

Electron Pump
High-Oxidation State
Photocatalysis
Single-Atom Catalysts
Water Splitting

ASJC Scopus subject areas

Catalysis
General Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/anie.202304634

Cite this

@article{bb0bff187e874dc6b4618a137badcd89,

title = "Isolated Electron Trap-Induced Charge Accumulation for Efficient Photocatalytic Hydrogen Production",

abstract = "The solar-driven evolution of hydrogen from water using particulate photocatalysts is considered one of the most economical and promising protocols for achieving a stable supply of renewable energy. However, the efficiency of photocatalytic water splitting is far from satisfactory due to the sluggish electron-hole pair separation kinetics. Herein, isolated Mo atoms in a high oxidation state have been incorporated into the lattice of Cd0.5Zn0.5S (CZS@Mo) nanorods, which exhibit photocatalytic hydrogen evolution rate of 11.32 mmol g−1 h−1 (226.4 μmol h−1; catalyst dosage 20 mg). Experimental and theoretical simulation results imply that the highly oxidized Mo species lead to mobile-charge imbalances in CZS and induce the directional photogenerated electrons transfer, resulting in effectively inhibited electron-hole recombination and greatly enhanced photocatalytic efficiency.",

keywords = "Electron Pump, High-Oxidation State, Photocatalysis, Single-Atom Catalysts, Water Splitting",

author = "Wenhuan Huang and Chenyang Su and Chen Zhu and Tingting Bo and Shouwei Zuo and Wei Zhou and Yuanfu Ren and Yanan Zhang and Jing Zhang and Magnus Rueping and Huabin Zhang",

note = "Funding Information: This work received financial support from the King Abdullah University of Science and Technology (KAUST), National Natural Science Foundation of China (22001156, 22271178), International Cooperation Key Project of Science and Technology Department of Shaanxi, China (2022KWZ‐06), the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province (20210602), Research project of Xi′an Science and Technology Bureau (2022GXFW0011), and Science and Technology New Star in Shaanxi Province (2023KJXX‐045). Funding Information: This work received financial support from the King Abdullah University of Science and Technology (KAUST), National Natural Science Foundation of China (22001156, 22271178), International Cooperation Key Project of Science and Technology Department of Shaanxi, China (2022KWZ-06), the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province (20210602), Research project of Xi′an Science and Technology Bureau (2022GXFW0011), and Science and Technology New Star in Shaanxi Province (2023KJXX-045). Publisher Copyright: {\textcopyright} 2023 Wiley-VCH GmbH.",

year = "2023",

month = jun,

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doi = "10.1002/anie.202304634",

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AU - Zhu, Chen

AU - Bo, Tingting

AU - Zuo, Shouwei

AU - Zhou, Wei

AU - Ren, Yuanfu

AU - Zhang, Yanan

AU - Zhang, Jing

AU - Rueping, Magnus

AU - Zhang, Huabin

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PY - 2023/6/19

Y1 - 2023/6/19

N2 - The solar-driven evolution of hydrogen from water using particulate photocatalysts is considered one of the most economical and promising protocols for achieving a stable supply of renewable energy. However, the efficiency of photocatalytic water splitting is far from satisfactory due to the sluggish electron-hole pair separation kinetics. Herein, isolated Mo atoms in a high oxidation state have been incorporated into the lattice of Cd0.5Zn0.5S (CZS@Mo) nanorods, which exhibit photocatalytic hydrogen evolution rate of 11.32 mmol g−1 h−1 (226.4 μmol h−1; catalyst dosage 20 mg). Experimental and theoretical simulation results imply that the highly oxidized Mo species lead to mobile-charge imbalances in CZS and induce the directional photogenerated electrons transfer, resulting in effectively inhibited electron-hole recombination and greatly enhanced photocatalytic efficiency.

AB - The solar-driven evolution of hydrogen from water using particulate photocatalysts is considered one of the most economical and promising protocols for achieving a stable supply of renewable energy. However, the efficiency of photocatalytic water splitting is far from satisfactory due to the sluggish electron-hole pair separation kinetics. Herein, isolated Mo atoms in a high oxidation state have been incorporated into the lattice of Cd0.5Zn0.5S (CZS@Mo) nanorods, which exhibit photocatalytic hydrogen evolution rate of 11.32 mmol g−1 h−1 (226.4 μmol h−1; catalyst dosage 20 mg). Experimental and theoretical simulation results imply that the highly oxidized Mo species lead to mobile-charge imbalances in CZS and induce the directional photogenerated electrons transfer, resulting in effectively inhibited electron-hole recombination and greatly enhanced photocatalytic efficiency.

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KW - High-Oxidation State

KW - Photocatalysis

KW - Single-Atom Catalysts

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M3 - Article

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SN - 1433-7851

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JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 25

M1 - e202304634

ER -

Isolated Electron Trap-Induced Charge Accumulation for Efficient Photocatalytic Hydrogen Production

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

UN SDGs

Access to Document

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